Method of conducting catalytic exothermic gaseous reactions



Nov. '24, 1931.

K. T. LARSON METHOD OF CONDUCTING CATALYTIC EXOTHERMIC GASEOUS REACTIONS Filed April 12. 1927 INVENTOR ATTORNEY loonrom'rroiv,'03WILMr GTONQE A AEE,4 oomgoIqArIoNo D L A E -is i ienii meaee w new or ana Patented Nov. 24, 1931' i r mmnop ori mimmqgxtmmmiflqr eofi whats;

' em ie' n fi tferir ile I1 'elq i u or ,1 usti v catalytie eizotl 'e a I I e es pne r jt bnst erp essu mi i pa t cul rly t t e ynth s (i am on rem V v Q i lfixtl fi fi ff ii fog i afii y m nl- 3 h atifyi g .ou he ce lyticieynt esis of 'ammoiiidi rider"pressure it isjd ecessaryto' r protect-the pressure-s stein ig wallfoflthe I reagti'on' apparatus fromjthe heaLt eyolved by 'the'freaetio'm j Otherwise the deteriorating efieet s of high tenipe'ratiire combined with the destructive action of thep mp ffss ed 113 (irogeiii may resultjiii Weakenmg ofth'e Wall he Po nt-0f s up i n." 'On Qd 0 relatiyelypooler mixture of nitrogen end.- hydrogen going tothe rea ctionhetyyeenthe pressure-sustaining wall I and the catalyst; The

eilt ig ous x u eis vthus mad t P ay a ub ere e i 'f hat itfr ms iies: he t 'immith ca a y t a d ei im n u yi f rm it protective screenfforf' the'press ufe' sustaini giwe h re y-k p h p ra ure of the latterbelow the point at whiehitsih'e chemical strength might' be impaired;

" jWhen, however, this method is appliedjto isyhthesis processes in the uneorribiiied nitrogen and hydrogemefter removal of an '39 moniabproduced' by the synthesie reaetioh, ie passed again oyer the sameor another 'body of eetll'yjs t, "considerable 'difiiculty is, ocea; 's'ioned by the small butapprecia ble ql aintities of ammonia ine itably remaining in theu Combined gases if the ammonia is removed by the methods customarilyused in practical operation; and particularly by eontlensetibi und r pressure. If the gases leaving the m5 inonia'rernoval system are' pes sed, eitherw'ith' or without m'ake-up'gasfi-i. e; fresh'hitrogen hydrogen mixture'to eompe 'seteyfor th'ehitrogen and hydrogen removed emmoniee into the reaction apliairatus between thje' pre's-, sure-sustaining Wall" 'andfthe catalyst 1 09115 tainer, the ammonia in the gases attacks the metal oi the pressure-sustaining Wall, probably "by forming a nitride." The 'corroding ectiohof this relatively small proportion of mmn is in iev g'o iie. even, t ela v y tiley sre e el tt la. @k; b construe '01 of fthe press r gs tgiin g described.

.re's'p'ect to detailsof apparatus and 'pfp fdh gp sa low temperature, tha n thtit offeither' thehy? Neither factory eol'litijoii 'ofthel problem;

A i t f e 5" d e s Wil ie-fee 1' parent e 8 het nv t dl iis bet ert d $twd y freferen to theytol'lovyi igspeoifieatior I In d n w th lr fienstheme suresustainirifg w all i s'Icooled. bythe mekejlip es di tinctffr in the g es lwhi lh hare 'preViouSlymaesed through 'theireacti'on endreeoyery' apparatiisgthat is," the fresh nitro 'gen-hydrogen;fifiixtureg after being" raised to the pres'slii'e at which the reectionis to be carried out, ispassed'into the eynthesis eppe ratus between the Catalyst container-and. {the pressure su'steinin'g wallyithe g ase's containilig 'residiial ammonia 'bei igthereafter fedd+ 7' ed toithe' make-'upgases" before the mixture pas s; into contact with the catalyst. I 'The pressure-sustaining Wall- 0211 thl'i'slheFfidig} qiiately protected from the heat ,of the' reaction land thepossibilityof deterioration of i the pressure-sustaining well by contact of ammonia'therewith'cerl'be avoided; y

Although the invention :is Js'usceptib'le fo'f embodiment in man different forms with One em t. 6 e i shq si iifcr p p se ie l st e in j i cmp. yin d' ew i g inw c r j- Theffigu ti'onofafi'apaf iii" t'us a aptedroithemtii iiat Y prises a metallic pressure-sustaining wall A,

5 enclosing a catalyst receptacle B which is, spaced therefrom to proyide Qt passage for' the cooling gas; rA heat exchangejcompar't- V mentTCper-inits warming the "gase goin to the reaction at the expense'o'f :thenot ga'ses rying ,out-thesynthesis' of ammonia the fresh compressed nitrogen-hydrogen mixture, i; e. ep nters... the pp ratus; through the inlet .Dlf Tt passes thence t r ugh the an u ar pa sage Rwher itp e ith ll zof.' t e wall B. "The mixture nters thgghgatge P hml g iHQ fiQE containing; gases e nlet 6 1 1 the apparatus through. t

' 'coillH QfItheheat eitchang 7 into fthe f coil: The gases 'then passthrough I the "conduitflJ wherein they are f urthei'fw'arnied' by heate'xchangewith. the catawith; Leavingfthe open? end: of J fthe fgases o flofw in thereyjerse' direction in contact with thecataly'st and'ther'e reacttofformiammonia. The asem i e o 'prdfl ts a Qa ly's'tj lirough it eorifices pag eve thecoil V H .'ana a Mit d W fli l j i app r u ri hf i ghiqu l The ga u p d t an; ethentreated for" ammonia remoyal by and hydr seflim x e, t ge r h t nempnd n' i ii m niai r u n d y ii a Pfimp "(hot fi ffid'lr iteri 'e ppa s thro h heiinlet" G- r V While j the; v apparatus; above. described is -a 99 11 1, 51%?if r .v p tlus nthe p a i e of theinvention, it will be obvious that, d epending "upon; the reactionto-be carried out and thecohditions under. which itis tobe efl'ect- V 9' t ed, itmaybeffounddesirable-to make certain modifications Thus-,ethe heatpexchangebee tWGenincomingand outgoing gasesj may :be accomplished Whollyor in part outside the reaction apparatusor may even in some cases be, dispensedwith. A1so,jthe amount of heat I removed from the catalyst by the gases in indirect ,contjact therewith may; be, :varied, dependingnponi the thermal, conductivity, of the metals'of which the wall B and the cong duittJ aremadep The-amount 0f heatfreand rf-the conduit J or in somei'cases by hmc natln the end t. J s -tl th gases in accordance lQfiYiIlgflie catalyst: Inlets Band ,G," and 'anoutletjl arej providedion-thejgases; ,In'car- ,5

imi erew thiq mam a ,t H g p ';Arjr'ioiig"'other iinportanthadvantages itipqr;

" :amount of heat from the catalyst throngli'the V irfiid ake pdoth rgases S i ,o

for capital investment n j'equlpment represwarmed theifl nt bing, gases roduet,1j 7

cooling in a condenser, ;and the uncoliibine'd' moved in this manner may also be controlled by the appl cation ofinsulationto the'wallB without preliminarily passing within and in indirect contact therewith. V a r The invention is not limited to the use of any specific catalyst nor to theemployment i i of any particular range of temperatures or pressures While especially; useful in the 'inyention'may also be advantageously applied other catalytic exothermic gaseous react 01 s inwhichithere'is formed;aiproductlike V 1y t0 tta kthe 'pressure-sustainingwall under'the conditions of operation.

' "ltwilll be apparnt from the 'ioregoing V that the inventionrepresents a practicable and efficient solutionfor" the problem of corrosion of pressure sustaining "walls-Lbyf-conif the reaction.

, i 'fi lh T 36 Q ordina m fi51i$ ,i iniisiy "steel ffor exampl where h therto e'xjpensiye corrosionfes 'stant alloys have'been vrequired.

' This a vantage is of l especial importance in View of'the'fact that iiiljth'e',comi'rler'cial oper ation of high pressure react'i'ons the' charge thereof;

thermi'c gaseous reactions under pressure, which vcolfipi'fises passing gases; free from ire: action productsf arol ildthe catalyst bod ;'e n yeloping thesairi ,lmihg ihgsuch gases there? aft'er with otherj gases ontaiain reaction j v products "and conductingjthemingled.igass 5 into direct contact with the catalyst? J I 2. The 'inethodjof eiie'cting. e (ganja; 1 7

synthesis" 0 ammoniafi'rom'iits elements under pressure, wh ch com r ses f pass ng} a mixtureof nitrogen and by rogen freejfrom 11o ammonia around the catalyst body, enye lopr' ing the same; mingling; s'uehimixtu're thereafter V with another gaseous mixture of nitrogen and hydrogen} containing ammonia and conducting thef mingled gases into 'direct'fcone tact withthe'catalys'tf efi'ectingicatalyt ic exo The lmethodfof 'therinic gas reactions under pressure; COHlPIlSQS sub ectinga gaseous mixturejde rivedfrom a previous reaction in contact with the catalyst to 'flfurther contact l gtherew 'ith; while passingagasifree fromlr'ea'ctionj prod5 ucts around the; catalys'ot 'bo dy', enveloping the, same, and, mingling; such gas, with the gaseous mixture? before ilatter fcontactg -12; v

witnithecatflyst;

synthesis ora nmqniarn om itselements'undel pressure, which 'comprises subjectinga 'as-j @0 atu sa ee aml hydi n ee-j v 1 V L 4. Thejmethodfof eifectingpthe Maya;

rived from a previous reaction in contact with the catalyst to further contact there-. with, while passing a gas free from ammonia around the catalyst body, enveloping the same, and mingling such gas with the gaseous mixture before the latter with the catalyst.

5. The process of effecting catalytic exo-v thermic gaseous reactions under pressure wherein a stream of make-up gas on its way to the catalyst is conveyed around the catalyst, envelopingthe same, while simultane-i ously passingdirectly to the catalyst gases which have already been subjected to the catalyst and from which reaction products havebeen partially removed.

6. The process of effecting the synthesis of ammonia under pressure wherein a stream of make-up hydrogen-mtrogenmixture on its way to the catalyst is conveyed around the catalyst body, enveloping the same, while" simultaneously passing directly to the catacontacts 1 afiix my signature. 

